Supercharging Metal-Organic Frameworks (SuperMOF)

The generation, transport, and lifetime of charge carriers is fundamental to the application of materials across all clean energy technologies. The oxidation and reduction behaviour of solids determines whether electrons and holes can be separated and collected in a solar cell, if a given solar fuel reaction will occur, or whether charge can be stored and later released in a battery or supercapacitor. While the rules for engineering the redox properties of inorganic and organic compounds are well established, hybrid organic-inorganic solids represent a new frontier that this project will explore. The flexibility of combining two distinct components in hybrid materials provides an infinite number of chemical and structural possibilities. However, there is no systematic approach established for designing compositions and configurations that match specific electronic criteria. I will focus on metal-organic frameworks (MOFs) based on ordered, and often porous, structures. The diversity of MOF building blocks and topologies provides access to an immense chemical space for engineering charge transfer pathways across multiple dimensions. SuperMOF will firmly establish the redox chemistry of MOFs. I will employ cutting-edge materials modelling techniques, including electronic structure simulations of massive frameworks, to: (i) develop a new redox theory that describes the unique behaviour of MOFs; (ii) construct design principles for engineering electron mobility and conductivity; (iii) model MOF photochemistry including heterointerfaces in solar energy devices. There are strong links with ongoing experimental activity to ensure rapid validation and testing of my predictions. The outcome will be a deep understanding of a new field of materials chemistry, the development of engineering principles for novel families of redox-active frameworks, and the support of a research group at the forefront of computational materials chemistry.